Giant optical orientation of exciton spins in lead halide perovskite crystals
Optical orientation of carrier spins by circularly polarized light is the basis of spin physics in semiconductors. Here, we demonstrate strong optical orientation of 85\%, approaching the ultimate limit of unity, for excitons in FA\(_{0.9}\)Cs\(_{0.1}\)PbI\(_{2.8}\)Br\(_{0.2}\) lead halide perovskit...
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creator | Kopteva, Natalia E Yakovlev, Dmitri R Yalcin, Eyüp Akimov, Ilya A Nestoklon, Mikhail O Glazov, Mikhail M Kotur, Mladen Kudlacik, Dennis Zhukov, Evgeny A Kirstein, Erik Hordiichuk, Oleh Dirin, Dmitry N Kovalenko, Maksym V Bayer, Manfred |
description | Optical orientation of carrier spins by circularly polarized light is the basis of spin physics in semiconductors. Here, we demonstrate strong optical orientation of 85\%, approaching the ultimate limit of unity, for excitons in FA\(_{0.9}\)Cs\(_{0.1}\)PbI\(_{2.8}\)Br\(_{0.2}\) lead halide perovskite bulk crystals. Time-resolved photoluminescence allows us to distinguish excitons with 60~ps lifetime from electron-hole recombination in the spin dynamics detected via coherent spin quantum beats in magnetic field. We reveal electron-hole spin correlations through linear polarization beats after circularly polarized excitation. Detuning of the excitation energy from the exciton resonance up to 0.5~eV does not reduce the optical orientation, evidencing clean chiral selection rules in agreement with atomistic calculations, and suppressed spin relaxation of electrons and holes even with large kinetic energies. |
doi_str_mv | 10.48550/arxiv.2305.10875 |
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Here, we demonstrate strong optical orientation of 85\%, approaching the ultimate limit of unity, for excitons in FA\(_{0.9}\)Cs\(_{0.1}\)PbI\(_{2.8}\)Br\(_{0.2}\) lead halide perovskite bulk crystals. Time-resolved photoluminescence allows us to distinguish excitons with 60~ps lifetime from electron-hole recombination in the spin dynamics detected via coherent spin quantum beats in magnetic field. We reveal electron-hole spin correlations through linear polarization beats after circularly polarized excitation. Detuning of the excitation energy from the exciton resonance up to 0.5~eV does not reduce the optical orientation, evidencing clean chiral selection rules in agreement with atomistic calculations, and suppressed spin relaxation of electrons and holes even with large kinetic energies.</description><identifier>EISSN: 2331-8422</identifier><identifier>DOI: 10.48550/arxiv.2305.10875</identifier><language>eng</language><publisher>Ithaca: Cornell University Library, arXiv.org</publisher><subject>Circular polarization ; Electron spin ; Electrons ; Excitation ; Excitons ; Holes (electron deficiencies) ; Lead compounds ; Linear polarization ; Metal halides ; Orientation ; Perovskites ; Photoluminescence ; Physics - Mesoscale and Nanoscale Physics ; Polarization (spin alignment) ; Polarized light ; Spin dynamics</subject><ispartof>arXiv.org, 2023-05</ispartof><rights>2023. This work is published under http://creativecommons.org/licenses/by-nc-nd/4.0/ (the “License”). 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Here, we demonstrate strong optical orientation of 85\%, approaching the ultimate limit of unity, for excitons in FA\(_{0.9}\)Cs\(_{0.1}\)PbI\(_{2.8}\)Br\(_{0.2}\) lead halide perovskite bulk crystals. Time-resolved photoluminescence allows us to distinguish excitons with 60~ps lifetime from electron-hole recombination in the spin dynamics detected via coherent spin quantum beats in magnetic field. We reveal electron-hole spin correlations through linear polarization beats after circularly polarized excitation. Detuning of the excitation energy from the exciton resonance up to 0.5~eV does not reduce the optical orientation, evidencing clean chiral selection rules in agreement with atomistic calculations, and suppressed spin relaxation of electrons and holes even with large kinetic energies.</description><subject>Circular polarization</subject><subject>Electron spin</subject><subject>Electrons</subject><subject>Excitation</subject><subject>Excitons</subject><subject>Holes (electron deficiencies)</subject><subject>Lead compounds</subject><subject>Linear polarization</subject><subject>Metal halides</subject><subject>Orientation</subject><subject>Perovskites</subject><subject>Photoluminescence</subject><subject>Physics - Mesoscale and Nanoscale Physics</subject><subject>Polarization (spin alignment)</subject><subject>Polarized light</subject><subject>Spin dynamics</subject><issn>2331-8422</issn><fulltext>true</fulltext><rsrctype>article</rsrctype><creationdate>2023</creationdate><recordtype>article</recordtype><sourceid>ABUWG</sourceid><sourceid>AFKRA</sourceid><sourceid>AZQEC</sourceid><sourceid>BENPR</sourceid><sourceid>CCPQU</sourceid><sourceid>DWQXO</sourceid><sourceid>GOX</sourceid><recordid>eNotj8tOwzAURC0kJKrSD2CFJdYpfuTayRJVUJCK2HQf3Ti2cAlxsN2q_XtCy-rMYjSaQ8gdZ8uyAmCPGI_-sBSSwZKzSsMVmQkpeVGVQtyQRUo7xphQWgDIGXlfexwyDWP2BnsaordDxuzDQIOj9mh8nmIa_ZCoH2hvsaOf2PvO0tHGcEhfPltq4ill7NMtuXYT7OKfc7J9ed6uXovNx_pt9bQpsAYolGt1zZwTNTO1BSG5kcwAZ0J3gG3V2tpZ3innOisESo5oailLpUzrlNJyTu4vs2fXZoz-G-Op-XNuzs5T4-HSGGP42duUm13Yx2H61IiKQyW1LkH-AtU0Wq4</recordid><startdate>20230518</startdate><enddate>20230518</enddate><creator>Kopteva, Natalia E</creator><creator>Yakovlev, Dmitri R</creator><creator>Yalcin, Eyüp</creator><creator>Akimov, Ilya A</creator><creator>Nestoklon, Mikhail O</creator><creator>Glazov, Mikhail M</creator><creator>Kotur, Mladen</creator><creator>Kudlacik, Dennis</creator><creator>Zhukov, Evgeny A</creator><creator>Kirstein, Erik</creator><creator>Hordiichuk, Oleh</creator><creator>Dirin, Dmitry N</creator><creator>Kovalenko, Maksym V</creator><creator>Bayer, Manfred</creator><general>Cornell University Library, arXiv.org</general><scope>8FE</scope><scope>8FG</scope><scope>ABJCF</scope><scope>ABUWG</scope><scope>AFKRA</scope><scope>AZQEC</scope><scope>BENPR</scope><scope>BGLVJ</scope><scope>CCPQU</scope><scope>DWQXO</scope><scope>HCIFZ</scope><scope>L6V</scope><scope>M7S</scope><scope>PIMPY</scope><scope>PQEST</scope><scope>PQQKQ</scope><scope>PQUKI</scope><scope>PRINS</scope><scope>PTHSS</scope><scope>GOX</scope></search><sort><creationdate>20230518</creationdate><title>Giant optical orientation of exciton spins in lead halide perovskite crystals</title><author>Kopteva, Natalia E ; Yakovlev, Dmitri R ; Yalcin, Eyüp ; Akimov, Ilya A ; Nestoklon, Mikhail O ; Glazov, Mikhail M ; Kotur, Mladen ; Kudlacik, Dennis ; Zhukov, Evgeny A ; Kirstein, Erik ; Hordiichuk, Oleh ; Dirin, Dmitry N ; Kovalenko, Maksym V ; Bayer, Manfred</author></sort><facets><frbrtype>5</frbrtype><frbrgroupid>cdi_FETCH-LOGICAL-a955-6fb790ff290c9e5231c30c51027d5ab8be9fe1d6ffde22a31aac933466cbf6673</frbrgroupid><rsrctype>articles</rsrctype><prefilter>articles</prefilter><language>eng</language><creationdate>2023</creationdate><topic>Circular polarization</topic><topic>Electron spin</topic><topic>Electrons</topic><topic>Excitation</topic><topic>Excitons</topic><topic>Holes (electron deficiencies)</topic><topic>Lead compounds</topic><topic>Linear polarization</topic><topic>Metal halides</topic><topic>Orientation</topic><topic>Perovskites</topic><topic>Photoluminescence</topic><topic>Physics - Mesoscale and Nanoscale Physics</topic><topic>Polarization (spin alignment)</topic><topic>Polarized light</topic><topic>Spin dynamics</topic><toplevel>online_resources</toplevel><creatorcontrib>Kopteva, Natalia E</creatorcontrib><creatorcontrib>Yakovlev, Dmitri R</creatorcontrib><creatorcontrib>Yalcin, Eyüp</creatorcontrib><creatorcontrib>Akimov, Ilya A</creatorcontrib><creatorcontrib>Nestoklon, Mikhail O</creatorcontrib><creatorcontrib>Glazov, Mikhail M</creatorcontrib><creatorcontrib>Kotur, Mladen</creatorcontrib><creatorcontrib>Kudlacik, Dennis</creatorcontrib><creatorcontrib>Zhukov, Evgeny A</creatorcontrib><creatorcontrib>Kirstein, Erik</creatorcontrib><creatorcontrib>Hordiichuk, Oleh</creatorcontrib><creatorcontrib>Dirin, Dmitry N</creatorcontrib><creatorcontrib>Kovalenko, Maksym V</creatorcontrib><creatorcontrib>Bayer, Manfred</creatorcontrib><collection>ProQuest SciTech Collection</collection><collection>ProQuest Technology Collection</collection><collection>Materials Science & Engineering Collection</collection><collection>ProQuest Central (Alumni Edition)</collection><collection>ProQuest Central UK/Ireland</collection><collection>ProQuest Central Essentials</collection><collection>ProQuest Central</collection><collection>Technology Collection</collection><collection>ProQuest One Community College</collection><collection>ProQuest Central Korea</collection><collection>SciTech Premium Collection</collection><collection>ProQuest Engineering Collection</collection><collection>Engineering Database</collection><collection>Publicly Available Content Database</collection><collection>ProQuest One Academic Eastern Edition (DO NOT USE)</collection><collection>ProQuest One Academic</collection><collection>ProQuest One Academic UKI Edition</collection><collection>ProQuest Central China</collection><collection>Engineering Collection</collection><collection>arXiv.org</collection><jtitle>arXiv.org</jtitle></facets><delivery><delcategory>Remote Search Resource</delcategory><fulltext>fulltext</fulltext></delivery><addata><au>Kopteva, Natalia E</au><au>Yakovlev, Dmitri R</au><au>Yalcin, Eyüp</au><au>Akimov, Ilya A</au><au>Nestoklon, Mikhail O</au><au>Glazov, Mikhail M</au><au>Kotur, Mladen</au><au>Kudlacik, Dennis</au><au>Zhukov, Evgeny A</au><au>Kirstein, Erik</au><au>Hordiichuk, Oleh</au><au>Dirin, Dmitry N</au><au>Kovalenko, Maksym V</au><au>Bayer, Manfred</au><format>journal</format><genre>article</genre><ristype>JOUR</ristype><atitle>Giant optical orientation of exciton spins in lead halide perovskite crystals</atitle><jtitle>arXiv.org</jtitle><date>2023-05-18</date><risdate>2023</risdate><eissn>2331-8422</eissn><abstract>Optical orientation of carrier spins by circularly polarized light is the basis of spin physics in semiconductors. Here, we demonstrate strong optical orientation of 85\%, approaching the ultimate limit of unity, for excitons in FA\(_{0.9}\)Cs\(_{0.1}\)PbI\(_{2.8}\)Br\(_{0.2}\) lead halide perovskite bulk crystals. Time-resolved photoluminescence allows us to distinguish excitons with 60~ps lifetime from electron-hole recombination in the spin dynamics detected via coherent spin quantum beats in magnetic field. We reveal electron-hole spin correlations through linear polarization beats after circularly polarized excitation. Detuning of the excitation energy from the exciton resonance up to 0.5~eV does not reduce the optical orientation, evidencing clean chiral selection rules in agreement with atomistic calculations, and suppressed spin relaxation of electrons and holes even with large kinetic energies.</abstract><cop>Ithaca</cop><pub>Cornell University Library, arXiv.org</pub><doi>10.48550/arxiv.2305.10875</doi><oa>free_for_read</oa></addata></record> |
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subjects | Circular polarization Electron spin Electrons Excitation Excitons Holes (electron deficiencies) Lead compounds Linear polarization Metal halides Orientation Perovskites Photoluminescence Physics - Mesoscale and Nanoscale Physics Polarization (spin alignment) Polarized light Spin dynamics |
title | Giant optical orientation of exciton spins in lead halide perovskite crystals |
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